OH-initiated degradation of several hydrocarbons in the atmosphere simulation chamber SAPHIR

Degradation of isoprene, m-xylene, n-octane, propene, and methacrolein by hydroxyl radicals has been studied in the simulation chamber SAPHIR under burden of trace gases as they are typical for the moderately polluted planetary boundary layer. Measured time series of the hydrocarbon mixing ratios and the OH concentrations were used to determine the rate constants. The hydrocarbons were measured with gas chromatography and proton transfer reaction mass spectrometry. OH was measured with the Jülich DOAS (differential optical absorption spectroscopy) instrument. In all cases except methacrolein good agreement was found with the reference rate constants taken from the Master Chemical Mechanism (MCM3.1). The data for methacrolein are consistent with the results of Karl et al. (J. Atmos. Chem 55, 2006, doi:) who reported a 12% smaller value. The degradation of hydrocarbons provides an independent method to analyse precision and accuracy of the OH measurements. A precision of better than 4% over a period of nearly 4 months was found. The accuracy is within the limitations given by the light absorption cross section of OH. Both results are consistent with earlier results by Hausmann et al. (J. Geophys. Res. 102:16011–16022, 1997).     

High resolution simulation of recent Arctic and Antarctic stratospheric chemical ozone loss compared to observations

Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1^∘ × 1^∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1^∘ × 1^∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO₃, N₂O, and NO _y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10⁻³ to 10⁻² cm⁻³) refines the agreement with in situ ozone, N₂O and NO _y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl₂O₂ absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl₂O₂ absorption cross-sections.     

Lagrangian Estimations of Ozone Loss in the Core and Edge Region of the Arctic Polar Vortex 1995/1996: Model Results and Observations

Ozone evolution and diabatic descent in the Arctic polar vortex in winter 1995/1996 was studied with a newly developed diabatic trajectory–chemistry model (DTCM). To study the chemical and dynamic evolution of the species in the polar vortex, 400 diabatic trajectories were calculated in the vortex core and edge region by using three-dimensional (3-D) wind data provided by the European Centre for Medium-Range Weather Forecasts (ECMWF). The averaged diabatic descending motion and ozone behavior were obtained for particles started from the core and from the edge region of the vortex. The difference in ozone-loss rates as well as the difference in descending rates between the vortex core and the vortex-edge region was not statistically significant. The average cumulative ozone loss of 65 ± 16% in the vortex core obtained from the model calculations was consistent with the estimates obtained with a different method (Match experiment). The model results for the vortex core were compared with those obtained using trajectories with the vertical winds calculated on the basis of radiative cooling rates as used by the SLIMCAT 3-D chemical transport model. Although the trajectories based on cooling rates exhibited lower descending rates than those based on 3-D analyzed wind data, the ozone behavior was similar for both types of trajectory. Ozonesonde data from two stations (Ny-Alesund in the vortex core and Yakutsk in the vortex edge) were compared with the model results. For Lagrangian estimation of the ozone loss at these stations, the descending rates obtained by the diabatic trajectory calculations were used. Good agreements were obtained between the model results and observations for both the vortex core and edge region. These results suggest that strong ozone depletion occurred not only in the core, but also in the edge region of the vortex, and that air masses from the mid-latitudes did not appreciably affect the degree of ozone depletion in this winter–spring period. The sensitivity of the model to different descending rates and to the presence of large nitric acid trihydrate (NAT) particles was also examined.     

DISTRIBUTIONS AND VARIATIONS OF SURFACE OZONE IN CHANGSHU, YANGTZE DELTA REGION*

Through one and half year continuous in-situ measurements,the distributions and variations of surface ozone and its precursors at a typical mixed agricultural and metropolitan area-Changshu,Yangtze Delta region,were studied.The preliminary analysis on the concentration levels and variations of surface ozone indicated the obvious seasonal and diurnal cycles during the experiment.The hourly averaged concentrations of surface ozone were high,in about 17% of total valid hours the surface ozone concentration exceeded 50 ppb,and in 22 days the hourly averaged ozone concentration was greater than 100 ppb.There were about 40% of the days in that the daily maximum 8-hour ozone concentration was greater than 50 ppb.The days with daily maximum 8-hour ozone concentration greater than 80 ppb were about 33 days that accounted for about 8% of the observational days.The variations of 5-day moving averaged ozone concentrations depended both on the weather conditions and on the changes of ozone in background atmosphere.Photochemical process had the significant impacts on ozone productions.     

IMPACTS OF OZONE CONCENTRATION AND EXPOSURE TIME CHANGES ON RICE YIELDS*

The impacts of O₃ concentration change on rice yields for different lengths of exposure time are studied by means of the OTC-1 open-top chamber.The resuhs indicate that when O₃ concentration increased from 50 ppb to 200 ppb during the time period of 20 to 80 days in the experiment,the rice yield was reduced by 6.78% to 33.72%.Two main influencing factors for rice yields are the increased O₃ concentration and the extended exposure time.Using a logarithm function to simulate the impacts of O₃ concentration on rice yields is better than using a the Weibull function.     

紫外差分吸收激光雷达测量平流层臭氧

我们研制了一台紫外差分吸收（UV-DIAL）激光雷达,用于18～45 km高度的平流层臭氧垂直廓线的长期监测。位于合肥的这一激光雷达于1996年8月全面建成并投入常规运行。本文将给出该激光雷达系统的结构和平流层臭氧测量数据处理。给出的一些测量结果和与其他手段测量结果的对比表明,该激光雷达对平流层臭氧能够进行可靠的测量。     

Column Observations of Stratospheric Gases at Søndre Strømfjord, Greenland During Winter 1994-1995

As part of the Second European Stratospheric Arctic and Mid-latitude Experiment (SESAME) field campaign, observations were made during the period from October 1994 to April 1995 at Søndre Strømfjord, Greenland (67°N, 53°W). Using a Fourier transform spectrometer, high resolution (0.06 cm-1) infrared spectra were recorded with the sun as a radiation source. Column amounts of trace gases including HCl, HF, HNO3, N2O and O3 are shown for five time periods during the course of the 1994-95 Arctic winter. Results are compared with lower stratospheric potential vorticity fields to describe variations in trace gas column amounts.     

Seasonal and interannual variations of upper tropospheric water vapor band brightness temperature over the global monsoon regions

The upper-troposphere water vapor (UTWV) band brightness temperature (BT) dataset derived from the High-resolution Infrared Radiation Sounder (HIRS) channel 12 of the National Oceanic and Atmospheric Admini-stration (NOAA) polar satellites from 1979 to 1995 is used to analyze the seasonal and interannual variations for the global monsoon regions. Results show that (i) there are three major regions where the UTWV band BT varies significantly with season, i.e., South Asia, the western coastal South-North America tropical region and the low-lati-tude African region; (ii) UTWV band BT clearly reveals the water vapor temporal / spatial features as well as the at-mospheric circulation structure over the low-latitude during the monsoon onset; and (iii) there is a remarkable rela-tionship between the interannua] variation of the UTWV band BT over the monsoon regions and the sea surface tem-perature anomaly in the eastern equatorial Pacific.     

Do Solar Flares Affect Total Ozone?

An analysis of total ozone from Hradec Králové (50.25°N, 15.21°E) and of radio wave absorption in the lower ionosphere at 1539 kHz (reflection point 50.3°N, 11.8°E) shows that there is no detectable effect of strong solar flares in total ozone, no correlation between total ozone and absorption on a day-to-day time scale, and that strong solar flares do not affect this correlation. Thus the long-term correlation of monthly average values (Alberca et al., 1996) is not reproduced on a day-to-day time scale, and the effects of strong geomagnetic storms in total ozone (Latovika et al., 1992; Mlch and Latovika, 1996) have no counterpart in effects of strong solar flares.     

GPSO3和Vaisala臭氧探空仪平行施放比对结果的初步分析

为促进中国大气臭氧高空探测业务化进程，中国科学院大气物理研究所和中国气象局监测网络司联合组织了对国产GPS数字化大气臭氧探空仪（GPSO3）和芬兰Vaisala 公司产大气臭氧探空仪(Vaisala)主要技术性能的比对。现场平行施放比对于2002年1月在北京进行，共施放了7对臭氧探空仪。对两类大气臭氧探空仪现场平行施放比对试验结果的分析表明，两种臭氧探空仪所获得的大气中臭氧浓度随高度的变化特征之间有很好的一致性。在12～27 km高度范围内，两种探空仪臭氧测值之间的相对误差平均在10％以内，而在10 km以下和27 km以上，GPSO3探空仪的臭氧测值偏高。本文介绍了比对方法，分析了两类探空仪对臭氧廓线某些特征值的比对结果并讨论了平行施放比对时气球升速的差异可能对臭氧测值带来的影响。